Organic solar cells (OSCs) have recently attracted considerable research interest. However, there is a mismatch between their optical absorption length and charge transport scale. Attempts to optimize both the optical and electrical properties of the photoactive layer of OSCs have inevitably resulted in demands for rationally designed device architecture. Plasmonic nanostructures have recently been introduced into solar cells to achieve highly efficient light harvesting. The remaining challenge is to improve OSC performance using plasmonic nanotechnology, a challenge taken up by the research reported in this thesis. I systematically investigated two types of plasmonic effect: localized plasmonic resonances (LPRs) and surface plasmonic resonances (SPRs).
Broadband plasmonic absorption is obviously highly desirable when the LPR effect is adopted in OSCs. Unfortunately, typical nanomaterials possess only a single resonant absorption peak, which inevitably limits the power conversion efficiency (PCE) enhancement to a narrow spectral range. To address this issue, I combined Ag nanomaterials of different shapes, including nanoparticles and nanoprisms. The incorporation of these mixed nanomaterials into the active layer resulted in wide band absorption improvement. My results suggest a new approach to achieving greater overall enhancement through an improvement in broadband absorption.
I also explored the SPR effect induced by a metal patterned electrode with two parts. Most reports to date on back reflector realization involve complicated and costly techniques. In this research, however, I adopted a polydimethylsiloxane (PDMS)-nanoimprinted method to produce patterned back electrodes in OSCs directly, which is a very simple and efficient technique for realizing high-performance OSCs in industrial processes. Besides, a remaining challenge is that plasmonic effects are strongly sensitive to light polarization, which limits plasmonic applications in practice. To address this issue, I designed three-dimensional patterns as the back electrode of inverted OSCs, which simultaneously achieved highly efficient and polarization-independent plasmonic OSCs.
In addition to investigating the two types of plasmonic effect individually, I also investigated their integrated function by introducing both LPRs and SPRs in one device structure. With the aim of achieving high-performance OSCs, I first demonstrated experimentally a dual metal nanostructure composed of Au nanoparticles (i.e. LPRs) embedded in the active layer and an Ag nanograting electrode (i.e. SPRs) as the back reflectors in inverted OSCs, which can generate a very strong electric field, in a single junction to improve the light absorption of solar cells. As a result, the PCE of the OSC reached 9.1%, making it one of the best-performing OSCs reported to date. In addition, as an important extension, I subsequently achieved tremendous near-field enhancement owing to multiple couplings, including nanoparticle-nanoparticle (LPR-LPR) couplings and nanoparticle-film (LPR-SPR) couplings, by designing a novel nanoparticle-film coupling system through the introduction of ultrathin monolayer graphene as a well-defined sub-nanogap between the Ag nanoparticles and Ag film. The graphene sub-nanogap is the thinnest nanogap (in atomic scale terms) to date, and thus constitutes a promising light-trapping strategy for improving future OSC performance.

Organic solar cells (OSCs) have recently attracted considerable research interest. However, there is a mismatch between their optical absorption length and charge transport scale. Attempts to optimize both the optical and electrical properties of the photoactive layer of OSCs have inevitably resulted in demands for rationally designed device architecture. Plasmonic nanostructures have recently been introduced into solar cells to achieve highly efficient light harvesting. The remaining challenge is to improve OSC performance using plasmonic nanotechnology, a challenge taken up by the research reported in this thesis. I systematically investigated two types of plasmonic effect: localized plasmonic resonances (LPRs) and surface plasmonic resonances (SPRs).
Broadband plasmonic absorption is obviously highly desirable when the LPR effect is adopted in OSCs. Unfortunately, typical nanomaterials possess only a single resonant absorption peak, which inevitably limits the power conversion efficiency (PCE) enhancement to a narrow spectral range. To address this issue, I combined Ag nanomaterials of different shapes, including nanoparticles and nanoprisms. The incorporation of these mixed nanomaterials into the active layer resulted in wide band absorption improvement. My results suggest a new approach to achieving greater overall enhancement through an improvement in broadband absorption.
I also explored the SPR effect induced by a metal patterned electrode with two parts. Most reports to date on back reflector realization involve complicated and costly techniques. In this research, however, I adopted a polydimethylsiloxane (PDMS)-nanoimprinted method to produce patterned back electrodes in OSCs directly, which is a very simple and efficient technique for realizing high-performance OSCs in industrial processes. Besides, a remaining challenge is that plasmonic effects are strongly sensitive to light polarization, which limits plasmonic applications in practice. To address this issue, I designed three-dimensional patterns as the back electrode of inverted OSCs, which simultaneously achieved highly efficient and polarization-independent plasmonic OSCs.
In addition to investigating the two types of plasmonic effect individually, I also investigated their integrated function by introducing both LPRs and SPRs in one device structure. With the aim of achieving high-performance OSCs, I first demonstrated experimentally a dual metal nanostructure composed of Au nanoparticles (i.e. LPRs) embedded in the active layer and an Ag nanograting electrode (i.e. SPRs) as the back reflectors in inverted OSCs, which can generate a very strong electric field, in a single junction to improve the light absorption of solar cells. As a result, the PCE of the OSC reached 9.1%, making it one of the best-performing OSCs reported to date. In addition, as an important extension, I subsequently achieved tremendous near-field enhancement owing to multiple couplings, including nanoparticle-nanoparticle (LPR-LPR) couplings and nanoparticle-film (LPR-SPR) couplings, by designing a novel nanoparticle-film coupling system through the introduction of ultrathin monolayer graphene as a well-defined sub-nanogap between the Ag nanoparticles and Ag film. The graphene sub-nanogap is the thinnest nanogap (in atomic scale terms) to date, and thus constitutes a promising light-trapping strategy for improving future OSC performance.

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eng

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The University of Hong Kong (Pokfulam, Hong Kong)

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HKU Theses Online (HKUTO)

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The author retains all proprietary rights, (such as patent rights) and the right to use in future works.

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This work is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License.